The effect of using small-scale, high surface area, nanoparticles to supplement polymer-conditioned wastewater sludge dewatering was investigated. Aerobically digested sludge and waste activated sludge sourced from the Hunter Valley, NSW, Australia, were tested with titanium dioxide nanoparticles. The sludge samples were dosed with the nanoparticles in an attempt to adsorb a component of the charged biopolymer surfactants present naturally in sludge. The sludge was conditioned with a cationic polymer. The dewatering characteristics were assessed by measuring the specific resistance to filtration through a modified time-to-filter testing apparatus. The solids content of the dosed samples was determined by a mass balance and compared to the original solids content in the activated sludge. Test results indicated that nanoparticle addition modified the structure of the sludge and provided benefits in terms of the dewatering rate. The samples dosed with nanoparticles exhibited faster water removal, indicating a more permeable filter cake and hence more permeable sludge. A concentration of 2–4% nanoparticles was required to achieve a noticeable benefit. As a comparison, the sludge samples were also tested with a larger particle size, powdered activated carbon (PAC). It was found that the PAC did provide some minor benefits to sludge dewatering but was outperformed by the nanoparticles. The solids content of the final sludge was increased by a maximum of up to 0.6%. The impact of the order sequence of particles and polymer was also investigated. It was found that nanoparticles added before polymer addition provided the best dewatering performance. This outcome was consistent with current theories and previous research through the literature. An economic analysis was undertaken to confirm the viability of the technology for implementation at a full-scale plant. It was found that, currently, this technology is unlikely to be favourable unless the nanoparticles can be sourced for a low cost.